Main set: I Was Made for You / Baby / I Got Your Number / Take It Back / Change Is Hard / Hold Me Thrill Me Kiss Me / Thieves / Turn to White / I Thought I Saw / You Really Got a Hold on Me / Stars Fell on Alabama / Ridin' in My Car / Don't Look Back / Magic Trick / Why Do You Let Me Stay Here / In the Sun / Never Wanted Your Love / Together / I Could Have Been Your Girl / Sweet Darlin'

Zooey Deschanel is either the most guileless of actresses – or she's one of the greatest of her generation. At the Hollywood Bowl on Sunday night, headlining the first of KCRW's World Festival Series as the distaff half of She & Him, the New Girl top-liner and star of movies such as (500) Days of Summer did not look like a celebrity.

Yes, she was glamorous in a backless blue gown, a ribbon ringing the back of her head like a garland, but for most of the duo's 70-minute set she stood at the microphone, arms stiffly by her side, looking out at the nearly sold-out Bowl with the wide-eyed blank stare of a kid giving her first public speech. If anything, she looks more nervous now than she did during S&H's first shows.

It serves her well, and certainly cuts down on the sweetness that threatened to overwhelm the 33-year-old last year, when those unfortunate "adorkable" promos for her Fox series threatened to turn this most confectionary of personalities into a cloying, one-dimensional sitcom star. (It doesn't hurt that the second season of New Girl was a vast improvement over the first.)

Deschanel's nerves here, in their second Bowl appearance but first headlining turn, made her seem more approachable, more human. That helps mark She & Him as more than just an actress' vanity project, and the deft mix of sunshine and melancholy that fills their recent Merge release Volume 3 (they've never put undue effort into their album titles) makes it hard to stay mad.

She loosened up, physically and vocally, when she sat at the piano for "Take It Back" and picked up a ukulele for "Thieves." She's not the most accurate of singers, though she has a natural sense of storytelling and pacing. "Change Is Hard" here had the blithe soul of Laura Nyro; she gave "Turn to White," a devastating finale to a relationship, a steely reserve; and she did a lovely job on a cover of the '50s chestnut "Hold Me Kiss Me Thrill Me," even if she couldn't quite nail the landing.

But her best performances were when she was alone on stage with musical partner M. Ward, taking on Smokey Robinson's "You Really Got a Hold on Me" and the classic "Stars Fell on Alabama" with visible intimacy and grace.

Ward is the perfect foil for Deschanel. His natural reticence, smart arrangements (even with an added string section, the sound remained airy) and love of artfully distressed sounds surround her with a mix that draws from a wide range of sophisticated pop: countrypolitan polish ("I Could Have Been Your Girl"), Brill Building songcraft ("Take It Back") and Beatles-esque melodicism ("In the Sun").

The staging, framed by small trees of lights and with the Chapin sisters offering matching dance moves while providing backing vocals, could have been something out of a '60s variety show. But Deschanel and Ward ended their set in more emotionally resonant fashion, serving up a sultry, spare version of "I Put a Spell on You." She certainly did.

Emmylou Harris and Rodney Crowell were also spellbinding, albeit in a different manner. Harris has an ethereal grace that is almost incomparable, yet the pairing's hour-long set was earthier than expected. The early going was a bit of business as usual: wondrous versions of songs she made famous alongside Gram Parsons ("Grievous Angel," "Wheels," "Love Hurts"), with Crowell's gruffer voice beautifully complementing Harris' purity, followed by a few tracks from their recently released album Old Yellow Moon.

Unlike the loose, scrabbled joy of their Troubadour appearance a few months back, this larger return felt almost too slick and professional. But two-thirds of the way into their set they brought out Albert Lee, lead guitarist for Harris & Crowell's 1970s Hot Band – and matters heated up. His solo on "Luxury Liner" stretched the song out even longer than expected, and the spark he lit continued burning as long as he remained on stage.

Even more surprising was the addition of violinist Mary Lou Simpson and her boyfriend, Incubus' Mike Einzinger. That Harris' and Crowell's conception of music can include a hard-rock guitarist is testament to their diverse talent.

M. Ward and Zooey Deschanel of She & Him perform at the Hollywood Bowl on Sunday. ARMANDO BROWN, FOR THE REGISTER
M. Ward and Zooey Deschanel of She & Him perform at the Hollywood Bowl on Sunday. ARMANDO BROWN, FOR THE REGISTER
M. Ward and Zooey Deschanel of She & Him perform at the Hollywood Bowl on Sunday. ARMANDO BROWN, FOR THE REGISTER
The world-famous Hollywood Bowl shell is lit up during She & Him's performance at the Hollywood Bowl on Sunday. ARMANDO BROWN, FOR THE REGISTER
Patty, Lisa and Lisa, from left, have fun at Sunday's She & Him concert at the Hollywood Bowl on Sunday. ARMANDO BROWN, FOR THE REGISTER
The Chapin sisters sing backup for She & Him at the Hollywood Bowl on Sunday. ARMANDO BROWN, FOR THE REGISTER
Peter and Giana of Tustin have fun at Sunday's She & Him concert at the Hollywood Bowl on Sunday. ARMANDO BROWN, FOR THE REGISTER

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